The ability to actively and dynamically control electronic states at ultrafast timescales opens up a wide range of potential applications across optoelectronics, quantum computing and sensing, energy conversion and storage, etc. Yet, achieving dynamic electronic manipulation via coherent phonons has posed a considerable challenge. Here, employing time-resolved high-harmonic generation (tr-HHG) spectroscopy, we demonstrate the manipulation of bandgap dynamics in a BaF2 crystal by coherent phonons. The tr-HHG spectrum perturbed by a triply degenerate phonon mode T2g exhibits simultaneously a remarkable two-dimensional (2D) sensitivity, i.e., in both intensity and energy domains. The dynamic compression and enhancement of the harmonics in the intensity domain showed a π/2 phase shift compared to the manifestation of shifts of the harmonics in the energy domain, an astounding example of a physical phenomenon being observed simultaneously in two different perspectives. We employed a quantum model incorporating the electron–phonon coupling to complement our experimental observations, successfully reproducing the results. In addition, we demonstrated complete control over the strength and initial phase of the coherent phonon oscillations by varying the incident electric field polarizations across different crystal orientations. Our findings lay a foundation for engineering the electronic structure through coherent phonons within the terahertz frequency and picosecond to nanosecond time regimes.
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